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JAMK University of Applied Sciences, Institute of Bioeconomy, Tuumalantie 17, FI-43130 Saarijrvi, Finland
Department of Biological and Environmental Science, University of Jyvskyl, P.O.Box 35, 40014, Finland
c
Department of Chemistry, University of Jyvskyl, P.O.Box 35, 40014, Finland
d
bo Akademi University, Strandgatan 2, FI-65100 Vaasa, Finland
b
art ic l e i nf o
a b s t r a c t
Article history:
Received 4 November 2014
Received in revised form
24 June 2015
Accepted 19 October 2015
Available online 11 November 2015
The compounds in stored woody biomass degrade as a result of chemical and/or biological processes
during storage. These processes produce gaseous emissions. Recent studies concerning gaseous emissions from wood pellet storages are reviewed herein. The applicability of the results from pellet research
to wood chips is discussed. Thorough scientic understanding on the storage phenomena of wood chips
is extremely important as the threat of climate change and the need to reduce greenhouse gas emissions
have led to an increased need to large scale wood chip storage to ensure supply. Typically the gases
produced from stored woody biomasses are carbon monoxide (CO), carbon dioxide (CO2), methane (CH4),
and other volatile hydrocarbons e.g. aldehydes and terpenes. CO2 and CH4 are greenhouse gases with
high global warming potential. Chemical degradation via auto-oxidation of fats and fatty-acids seems to
be the dominant mechanism for off-gassing from stored wood pellets, whereas biological processes are
mainly responsible for the gaseous emission from wood chips. In conned storage spaces gaseous
emissions may lead to oxygen depletion. Oxygen depletion together with a high CO concentration poses
a serious health risk for those working in such conditions. The degradation processes also result in dry
matter losses and in spontaneous heating and in the worst case, especially in large piles, spontaneous
ignition of the stored material. Thorough and systematic scientic studies on degradation processes and
their effects are needed in order to understand and minimise risks from large scale wood chips storage to
human health, environment and property.
& 2015 Elsevier Ltd. All rights reserved.
Keywords:
Emissions
Degradation
Risks
Biomass storage
Wood pellets
Wood chips
Contents
1.
2.
3.
4.
Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 377
Wood pellet storage . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 377
2.1.
Storage halls and silos . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 377
2.2.
Storage during transportation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 377
Gases typically emitted from pellet storages, their effects and risks . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 378
3.1.
Experimental methodology used in woody biomass storage studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 378
3.2.
Gases emitted from wood pellet storage and their risks . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 378
3.2.1.
Carbon monoxide (CO) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 378
3.2.2.
Carbon dioxide (CO2) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 378
3.2.3.
Methane (CH4) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 379
3.2.4.
Nitrous oxide (N2O) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 379
3.2.5.
Other volatile organic compounds . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 379
Results from pellet off-gassing studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 379
4.1.
Gas concentrations in pellet storages . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 379
4.2.
Types of gases emitted from pellet storages and their safety data . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 380
n
Corresponding author at: JAMK University of Applied Sciences, Institute of Bioeconomy, Tuumalantie 17, FI-43130 Saarijrvi, Finland. Tel.: 358 50 360 1968;
fax: 358 14 260 2321.
E-mail address: ealakosk@gmail.com (E. Alakoski).
http://dx.doi.org/10.1016/j.rser.2015.10.021
1364-0321/& 2015 Elsevier Ltd. All rights reserved.
377
4.3.
Factors affecting gaseous emissions from pellet storages . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 380
Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 381
5.1.
Storage of wood pellets compared to wood chips . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 381
5.2.
Factors and risks affecting large scale storage of wood chips . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 381
5.3.
Risks from storage of wood chips to property . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 381
5.3.1.
The effect of the pile size in spontaneous heating of storage piles. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 381
5.3.2.
Factors affecting spontaneous ignition of large wood chips piles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 382
5.4.
Health risks from storage of woody biomass . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 382
5.5.
Environmental risks from storage of woody biomass . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 382
6. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 382
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 382
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 382
5.
1. Introduction
The threat of climate change and the need to reduce greenhouse gas emissions have led to an increase in the demand and
use of biomass in energy generation. In order to ensure supply, this
means increasing in the amounts of biomass in storage for
extended time periods. In areas with high heating demand during
winter time e.g. in the northern coniferous forest belt this typically
means woody biomass such as stem wood, wood chips and wood
pellets.
Gaseous emissions are produced during storage of woody
biomass [13]. The gases produced are typically greenhouse gases
and present serious risks for people entering enclosed storages.
Chemical and biological degradation processes are responsible for
these emissions. The processes leading to gaseous emissions also
produce dry matter losses, deterioration of mechanical properties
and spontaneous heating in the stored material [46]. These processes and their effects need to be thoroughly understood in order
to minimise the risks produced.
During the last fteen years wood pellet production, storage
and use has seen a rapid increase. Some serious accidents with
fatalities have also happened in pellet storages [7,8]. Preventing
such accidents from happening has been the main motivation of
several studies on gaseous emissions (off-gassing) from wood
pellets [1,2,9]. On the other hand, similar studies on gaseous
emission from stored wood chips are almost non-existent. Fears of
re hazards from spontaneous heating in the stored material and
of dry matter losses are currently the main factors limiting the
storage of wood chips in large piles. Herein it is postulated that as
both pellets and chips are produced from woody biomass the
phenomenology during storage of both is similar and therefore
signicant insight to wood chip storage phenomena can be gained
by considering pellet studies. This paper reviews pellet off-gassing
studies and tries to reect on the similarities in wood pellet and
wood chip degradation phenomena. The purpose of this work is to
provide a foundation for further research on the degradation
processes on-going in wood chip storages. The ultimate goal of
such experimental research is the development of new and safe
methods to store wood chips in large piles for extended time
periods.
378
Table 1
Atmospheric life-times, global warming potentials (GWPs) and radiative forcing
(RF) effects of CO2, CH4 and N2O [19].
Gas
Lifetime (a)
GWP 20 a
GWP 100 a
GWP 500 a
RF (W m 2)
CO2
CH4
N2O
100200
12
114
1
72
298
1
25
289
1
7.6
153
1.66
0.48
0.16
379
380
Table 2
CO, CO2, CH4, aldehyde and terpene concentrations measured from wood pellet storages.
Compound
Storage time
T (C)
Amount (g)
C (mg m 3)
Environment
Additional information
Ref.
CO
8 wa
8w
6w
6w
79 w
?
18 hb
56 dc
56 d
42 d
42 d
79 w
56 d
56 d
42 d
42 d
79 w
18 h
18 h
?
3h
?
?
20
40
20
40
525
?
?
20
40
20
40
525
20
40
20
40
525
?
?
?
?
1719
?
800
800
1200
1200
3000M
30M
6M
800
800
1200
1200
3000M
800
800
1200
1200
3000M
?
6M
30M
?
7000M
30M
640
16,700
400
16,300
1700 17,000
4900
1237 10
9300
65,900
3900
55,600
5400 31,300
90
670
5
200
50640
111 732
987 4
309
3.6
14.719.2
52
35/87
Laboratory
Laboratory
Laboratory
Laboratory
Ocean vessels
Domestic
Domestic
Laboratory
Laboratory
Laboratory
Laboratory
Ocean vessels
Laboratory
Laboratory
Laboratory
Laboratory
Ocean vessels
Industrial
Domestic
Domestic
Industrial
Industrial
Domestic
Canadian pine
Canadian pine
European Pinus sylvestris
European Pinus sylvestris
Five intercontinental transportations
Conc. exceeded measurement range
[15]
[15]
[15]
[15]
[13]
[6]
[1]
[15]
[15]
[15]
[15]
[13]
[15]
[15]
[15]
[15]
[13]
[1]
[1]
[6]
[1]
[6]
[6]
CO2
CH4
Aldehydes
Terpenes
a
b
c
9100/
No limit
/42
For hexanal
140/180
For turpentine
Canadian pine
Canadian pine
European Pinus sylvestris
European Pinus sylvestris
Five intercontinental transportations
Canadian pine
Canadian pine
European Pinus sylvestris
European Pinus sylvestris
Five intercontinental transportations
w weeks.
h hours.
d days.
Table 3
Volatile organic compounds emitted from pellet storages and their classications.
Classication
Compound (CAS#)
Classication
Compound (CAS#)
Alkane
Alkane
Alkene
Alkene
Aldehyde
Aldehyde
Aldehyde
Aldehyde
Aldehyde
Aldehyde
Aldehyde
Aldehyde
Unsaturated aldehyde
Unsaturated aldehyde
Unsaturated aldehyde
Pentane (109-66-0)
Heptane (142-82-5)
Ethene (74-85-1)
Propene (115-07-1)
Ethanal (75-07-0)
Butanal (123-72-8)
Pentanal (110-62-3)
Hexanal (66-25-1)
Heptanal (111-71-7)
Nonanal (124-19-6)
Decanal (112-31-2)
2-Ethylhexanal (123-05-7)
Acroleine (107-02-8)
Crotonaldehyde (4170-30-3)
2-Heptenal (2463-63-0)
Aromatic aldehyde
Ketone
Alcohol
Alcohol
Alcohol
Terpene
Terpene
Terpene
Terpene
Organic acid
Organic acid
Organic acid
Organic acid
Aromatic hydrocarbon
Aromatic hydrocarbon
Benzaldehyde (100-52-7)
Acetone (67-64-1)
Methanol (67-56-1)
Butanol (75-65-0)
Isopropanol (67-63-0)
-Pinene (2437-95-8)
-Pinene (-)
Carene (13466-78-9)
D-Limonene (5989-27-5)
Formic acid (64-18-6)
Pentanoic acid (109-52-4)
Hexanoic acid (109-52-4)
Caproic acid (142-62-1)
Toluene (108-88-3)
Methyl-isopropylbenzene (99-87-6)
4.2. Types of gases emitted from pellet storages and their safety data
A large variety of NMVOCs have been detected from different
types of pellet storages. NMVOCs emitted from pellet storages can
be e.g. alkanes, alkenes saturated, unsaturated and aromatic
aldehydes, ketones, terpenes, alcohols and organic acids [1,9,18].
The compounds detected from pellet storages, their CAS numbers,
and chemical classications are given in Table 3.
The concentrations of the compounds shown in Table 3 vary
several orders of magnitude depending e.g. on the compound,
storage type and measurement location in the storage [1,9,18]. For
simplicity the concentrations are omitted. According to their
chemical safety data sheets, many of these compounds are classied as highly ammable and may thus play a role in the selfignition phenomenon. A systematic study is needed to clarify the
role of gases in self-ignition of stored material of biological origin.
However, the large amount of different compounds detected
illustrates the complexity of off-gassing from storage and the
challenge of such studies. For comparison, according to a qualitative study by He et al. [44] the major chemical compounds emitted
381
2. Off-gassing from pellet storages seem to be a result predominantly of chemical processes. The monotonous increase of gas
production Kuang et al. observed as a function of increased
temperature is an indication of this [20]. If microbial action
would be responsible gas production there would be an
increase to a certain level and then a decline as bacteria and
fungi perish [45].
3. Auto-oxidative degradation of fats and fatty acids is postulated to
be the principal process responsible for CO emissions from pellets
[1,20]. Lower fatty acid content in the raw material leads to lower
aldehyde and ketone emissions, e.g. these emissions are signicantly lower from spruce pellets than from pine pellets, as spruce
typically contains less fatty acids than pine [46].
4. According to measurements by Svedberg et al. CO concentrations measured from wood chip and timber transportation are
signicantly lower than those measured from pellet transportation [43]. This is an evidence of microbial action as microbial
decomposition favours the production of CO2 over CO. The
results from microbial activity measurements in colonyforming units per gram of material conrm this. The bacterial
and fungal activities in samples of dry or wet wood pellets were
o 13 cfu g 1 and o13 cfu g 1, respectively and in comparison
in freshly produced wood chips 9.4 105 cfu g 1 and
7.1 105 cfu g 1, respectively [43]. The reason behind this
drastically lower microbial activity in pellets is evidently the
dehydration at high temperatures. High temperature and low
humidity are environmental conditions that do not favour
microbial activity [43,47].
5. An increase in ambient relative humidity increases emissions [20].
6. The availability of oxygen increases peak off-gas emissions [20].
7. Predominant VOCs emitted from freshly produced sawdust (the
typical raw material used for pellet production) are terpenes.
Most of the terpenes are emitted in the rst few weeks of storage, and simultaneously hexanal production from sawdust
starts to increase [10].
8. In pellets made from fresh sawdust Hexanal off-gassing peaks a
few weeks after pellet production and starts to gradually
diminish to low levels after a few months in storage [10,48].
When aged sawdust is used as a raw material Hexanal production remains high up to half a year [48].
9. The physical handling of pellets e.g. repeated loading and
unloading of pellets increases instantaneous emissions [8,18].
5. Discussion
5.1. Storage of wood pellets compared to wood chips
There are several risks involved in the storage of materials of
biological origin. Chemical and biological degradation in stored
biomass leads to emission of volatile gases that introduce serious
health risks for employees. The risks are especially high when
biomass is stored in conned spaces. Storage in enclosed spaces
leads to accumulation of emitted gases and oxygen depletion. The
degradation processes may also lead to dry matter losses and
spontaneous heating in the storage piles. The worst case scenario
is self-ignition of the storage pile. When woody biomass is stored,
5.2. Factors and risks affecting large scale storage of wood chips
The material losses and the risk of res due to spontaneous
heating are signicant with large-scale wood chip storage. There
are several complicating factors affecting wood chip storages.
Wood chips undergo no pre-treatments prior to chipping, except
the natural drying of the raw material in outdoor conditions.
Wood chips have a large surface area which facilitates microbial
colonisation [47]. Forest residues and bark typically used as a raw
material for chips contain high concentrations of minerals and
inorganic elements that may enhance microbial activity. Storage
outdoors in varying weather conditions may induce moisture and
temperature gradients that probably affect the diffusion of oxygen
and other gases in the pile. Storage outdoors also increases the risk
of microbial colonisation from atmospheric deposition by rain,
transportation by wind or immigration e.g. from the ground below
the pile [47]. Considering the aforementioned factors it is evident
that microbial activity plays a major role in degradation processes
happening in a wood chip pile. Of course as chemical reactivity
increases with increasing temperatures it is highly likely that
chemical processes are enhanced as the temperature inside the
storage pile increases. The key inputs, factors and the risks produced during long term large-scale wood chip storage are summarised in Fig. 1.
5.3. Risks from storage of wood chips to property
382
Biological input
Fungal and bacterial action
and respiration
Aerobic and anaerobic
degradation of wood
constituents; cellulose,
hemicellulose, lignin
Physical input
RISKS
Pile size
Chemical input
Oxidation reactions
Autooxidation of fats
Exothermic reactions
Availability of oxygen
Mineral content
pH
Environmental input
Ambient temperature
Rainfall, Snowfall,Wind
Transportation of microbes
and material
Pile base effects:soil/material
type, slope, shape
Fig. 1. A scheme summarizing the key inputs and factors leading to risks on human
health, the environment and property during long-term, large scale storage of
wood chips.
The focus of pellet storage gas emission studies has been on CO,
CO2, CH4 and NMVOC s, their effects on human health and related
employee safety issues. Magelli et al. published a study on the
environmental impact of greenhouse gas emissions from pellet
production and transportation [17]. Their life-cycle emission
assessment fails to include GHG emissions from storage. The most
signicant greenhouse gasses emitted from pellet storages are CO2
and CH4. No studies on N2O emissions from pellet storages were
found from literature. Of course compared to GHG emissions
produced from transporting pellets from e.g. Canada to Europe the
emissions from storage are bound to be insignicant as the fuel
consumed in production and transportation corresponds up to 40%
of energy content of the pellets being transported [17]. However, a
simple way to make a clear reduction in the life-cycle emissions of
pellets would be to use them near the production sites. In such
case reduced emissions from pellet transportation would increase
the relative signicance of GHG emissions from storage. This is
especially so as some storage conditions may favour the production of CH4 and N2O, compounds with high GWPs. With longduration storage of wood chips the emissions from storage are
more important as wood chips cannot be transported in an economically viable way over long distances.
6. Conclusions
Due to the threat of climate change and with increasing oil
prices there is need for increasing the use of biomasses for energy.
With increasing use of biomasses for energy there comes also the
increasing need for storage of woody fuels especially wood chips.
However, there are apparent risks involved in large-scale storage
of wood chips. These include; the risks of res, due to spontaneous
warming and ignition; risk of the reduction of fuel quality and dry
matter losses; human health risks arising from gaseous emission
produces and the presence of pathogenic microbes and environmental risks from the emissions of greenhouse gases. These risks
arise from complex biological and physicochemical degradation
processes ongoing in large wood chip storage piles. Currently there
is an apparent lack of scientic understanding on factors affecting
these processes. More research and a thorough understanding of
these processes are needed for the development of new and safe
storage procedures for large scale storage of wood chips.
Acknowledgements
The writing of this manuscript was supported in part by the
BIOCLUS (FP7/Regions of Knowledge/245438) -project, Fortum
Foundation and The Foundation for Research of Natural Resources
in Finland.
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